The development of two-dimensional (2D) layered metal–organic frameworks (MOFs) through precise molecular-level design and synthesis has emerged as a prominent research endeavor. However, the utilization of MOFs in their pristine form as electrodes for supercapacitors poses a significant challenge due to their limited tolerance in alkaline environments. To address these issues, we have developed Co- and Cu-based pillar-layered MOFs by regulating the structure of their inner layers through introducing an alkaline N-containing “pillar” to enhance the performance of alkaline supercapacitor electrodes. From the microstructure study and theoretical calculation, the high-density redox centers and efficient chemical bonding modes of Co-MOF determine a unique electron conduction pathway, resulting in excellent energy storage performance. This study underscores the significance of chemical bonding modes and active-site distribution in enhancing the energy storage capabilities of pillar-layered MOFs in alkaline environments, presenting a promising approach for the development of high-performance MOF-based materials for supercapacitor applications.

中文翻译：

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用于高性能碱性超级电容器的具有丰富活性位点分布的柱支撑二维层状 MOF


通过精确的分子水平设计和合成开发二维（2D）层状金属有机框架（MOF）已成为一项突出的研究工作。然而，由于其在碱性环境中的耐受性有限，利用原始形式的 MOF 作为超级电容器的电极提出了重大挑战。为了解决这些问题，我们开发了钴基和铜基的柱状层状MOF，通过引入碱性含氮“柱”来调节其内层结构，以增强碱性超级电容器电极的性能。从微观结构研究和理论计算来看，Co-MOF的高密度氧化还原中心和高效的化学键合模式决定了独特的电子传导路径，从而产生优异的储能性能。这项研究强调了化学键合模式和活性位点分布在增强碱性环境中柱层MOF储能能力方面的重要性，为开发用于超级电容器应用的高性能MOF基材料提供了一种有前景的方法。